含有离子型 4,4-联吡啶鎓基团并用钯纳米粒子装饰的高有序周期性介孔有机硅材料:关于纳米反应器的建议

IF 5.2 2区 化学 Q1 CHEMISTRY, APPLIED Catalysis Today Pub Date : 2024-08-27 DOI:10.1016/j.cattod.2024.115016
Cezar A. Didó, Carlos D.G. Caneppele, Douglas S. Charqueiro, Eliana W. de Menezes, Leliz T. Arenas, Tania M.H. Costa, Edilson V. Benvenutti, Marcelo P. Gil
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引用次数: 0

摘要

成功制备了一种含有阳离子 4,4-联吡啶鎓基团的周期介孔有机硅(PMO),其含量为 0.25 mmol g-1,相当于 11.5 w/w%。设计这种材料的目的是使离子基团作为 PdCl42- 阴离子络合物的锚定剂,其含量远远低于现有的阳离子位点(3 摩尔%和 15 摩尔%)。随后,钯络合物被原位还原,得到稳定的钯纳米粒子(PdNP)。一系列表征结果表明,PMO 材料的壁具有六角形堆积的圆柱形形态,即使在装饰了 PdNP 之后,也能产生尺寸分布窄、表面积高的有序孔隙。考虑到这种材料的化学位点和密闭环境具有空间均匀性,因此有望成为一种高效的纳米反应器。为了评估钯位点的可用性,该材料被用作对硝基苯酚模型还原反应的催化剂。尽管本研究的催化剂具有与其他已报道系统相当的活性,但它却是文献中发现的钯/对硝基苯酚摩尔比最低的催化剂,令人印象深刻。
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Highly ordered Periodic Mesoporous Organosilica material containing the ionic 4,4-bipyridinium group and decorated with palladium nanoparticles: A proposal for nanoreactor

A Periodic Mesoporous Organosilica (PMO) containing the cationic 4,4-bipyridinium group, presenting 0.25 mmol g−1 that corresponds to 11.5 w/w%, was successfully prepared. This material was designed to have the ionic group acting as anchoring agent of PdCl42- anion complex, in a much lower amount than the available cationic sites (3 and 15 molar%). Subsequently, the palladium complex was in situ reduced to obtain stabilized palladium nanoparticles (PdNP). The ensemble of characterization results showed that the PMO material walls have a cylindrical morphology with hexagonal packing, generating well-ordered pores with a narrow size distribution and high surface area, even after being decorated with PdNP. This material is a candidate to be an efficient nanoreactor considering that it contains spatial uniformity in its chemical sites and confined environment. Aiming to evaluate the availability of palladium sites, the material was used as a catalyst in the reduction of p-nitrophenol model reaction. Although the catalyst of the present study has a comparable activity with other already reported systems, it presents the impressive lowest molar palladium/p-nitrophenol ratio found in literature.

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来源期刊
Catalysis Today
Catalysis Today 化学-工程:化工
CiteScore
11.50
自引率
3.80%
发文量
573
审稿时长
2.9 months
期刊介绍: Catalysis Today focuses on the rapid publication of original invited papers devoted to currently important topics in catalysis and related subjects. The journal only publishes special issues (Proposing a Catalysis Today Special Issue), each of which is supervised by Guest Editors who recruit individual papers and oversee the peer review process. Catalysis Today offers researchers in the field of catalysis in-depth overviews of topical issues. Both fundamental and applied aspects of catalysis are covered. Subjects such as catalysis of immobilized organometallic and biocatalytic systems are welcome. Subjects related to catalysis such as experimental techniques, adsorption, process technology, synthesis, in situ characterization, computational, theoretical modeling, imaging and others are included if there is a clear relationship to catalysis.
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